Aqueous Reaction Kinetics And Secondary Organic Aerosol Formation From Atmospheric Phenol Oxidation
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Aqueous Reaction Kinetics and Secondary Organic Aerosol Formation from Atmospheric Phenol Oxidation
Author | : Jeremy Daniel Smith |
Publisher | : |
Total Pages | : |
Release | : 2014 |
Genre | : |
ISBN | : 9781321609912 |
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Organic aerosols (OA) are a dominant fraction of particulate mass in the atmosphere, and much is secondary in nature. Secondary organic aerosol (SOA) is formed in the atmosphere from volatile organic compound precursors. Traditional SOA formation pathways involve primarily gas-phase processes: Oxidation reactions of organic gases result in low-volatility products that condense to the particulate phase, increasing aerosol mass. However, in recent years heterogeneous processes, including aqueous reactions, have gained more attention as gas-phase processes often fail to accurately predict observed mass loadings of aerosol in the atmosphere. Aqueous SOA formation is the result of a volatile organic species partitioning to the aqueous phase (clouds, fogs, aqueous aerosols), where they are chemically converted into a non-volatile species that remains in the particulate phase upon water evaporation. In this work we explore the aqueous chemical reaction kinetics and the SOA formation potential of phenols, which are released in large quantities from biomass combustion. Phenols are a broad class of organic compounds with intermediate volatilities (102 - 106 [mu]g m−3 at 20°C) and moderate to high Henry's Law Constants (103 - 109M atm−1), indicating significant partitioning to atmospheric aqueous phases. We begin in chapters 2 and 3 by investigating the aqueous oxidation of the compounds phenol (compound with formula C6H5OH), guaiacol (2-methoxyphenol), syringol (2,6-dimethoxyphenol), and three dihydroxybenzenes (catechol, resorcinol, hydroquinone). For each phenol we examined reactions with two oxidants: hydroxyl radical (*OH) and the triplet excited state of 3,4-dimethoxybenzaldehyde, which is also emitted from biomass combustion. Triplet excited states (3C*) have been widely studied in surface waters (oceans and lakes) but are a novel oxidation pathway in atmospheric aqueous phases. The precursors for triplet excited states are essentially brown carbon: organic molecules high amoutns of conjugation (or nitrogen hetero atoms) that can absorb solar radiation, resulting in an excited molecule with a high oxidative potential. We find that the 3C*-mediated aqueous oxidations of phenols are rapid and can dominate over *OH at low pH (
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